In situ tracer tests to determine retention properties of a block scale fracture network in granitic rock at the Aspö Hard Rock Laboratory, Sweden

Experiments were conducted at the Asp? Hard Rock Laboratory in order to improve the understanding of radionuclide retention properties of fractured crystalline bedrock in the 10-100 m scale (TRUE Block Scale Project, jointly funded by ANDRA, ENRESA, Nirex, JNC, Posiva and SKB). A series of tracer experiments were performed using sorbing tracers in three different flow paths. The different flow paths had Euclidian lengths of 14, 17 and 33 m, respectively, and one to three water conducting structures. Four tests were performed using different cocktails made up of radioactive sorbing tracers (22,24Na+, 42K+, 47Ca2+, 85Sr2+, 83,86Rb+, 131,133Ba2+ and 134,137Cs+). For each tracer injection, the breakthrough of sorbing tracers was compared to the breakthrough of a conservative tracer, 82Br-, 131I-, HTO and 186ReO4-, respectively. In the two longer flow paths, no breakthrough of 83Rb+ and 137Cs+ was observed after 8 months of pumping. Selected tracer tests were subject to basic modelling in which a one-dimensional (1D) advection-dispersion model, including surface sorption, and an unlimited matrix diffusion were used for the interpretation of the results. The results of the modelling indicated that there is a slightly higher mass transfer into a highly porous material in the block-scale experiment compared with in situ experiments performed over shorter distances and significantly higher than what would have been expected from laboratory data obtained from studies of the interactions in nonaltered intact rock.     

Soil to leaf transfer factor for the radionuclides ²²⁶Ra, ⁴⁰K, ¹³⁷Cs and ⁹⁰Sr at Kaiga region, India

Transfer factors are the most important parameters required for mathematical modeling used for environmental impact assessment of radioactive contamination in the environment. In this paper soil to leaf transfer factor for the radionuclides ⁴⁰K, ²²⁶Ra, ¹³⁷Cs and ⁹⁰Sr is estimated for Kaiga region in Karnataka state, India. Among the plants in which study is carried out, ²²⁶Ra, ⁴⁰K, ¹³⁷Cs and ⁹⁰Sr activity in leaves of herbaceous plants is higher than that of tree leaves. Soil to leaf transfer factor for ²²⁶Ra, ⁴⁰K, ¹³⁷Cs and ⁹⁰Sr was found to be in the range of 0.03-0.65, 0.32-8.04, 0.05-3.03 and 0.42-2.67 respectively.     

Fractionation of radionuclide species in the environment

Naturally occurring and artificially produced radionuclides in the environment may be present in different physico-chemical forms (i.e., radionuclide species) varying in size (nominal molecular mass), charge properties and valence, oxidation state, structure and morphology, density, degree of complexation, etc. Low molecular mass (LMM) species are believed to be mobile and potentially bioavailable, while high molecular mass (HMM) species such as colloids, polymers, pseudocolloids and particles are considered inert. Due to time-dependent transformation processes such as mobilisation of radionuclide species from solid phases or interactions of mobile and reactive radionuclide species with components in soils and sediments, the original distribution of radionuclides deposited in ecosystems will change over time. To assess the environmental impact from radionuclide contamination, information on radionuclide species deposited, interactions within affected ecosystems and the time-dependent distribution of radionuclide species influencing mobility and biological uptake is essential. The development of speciation techniques to characterize radionuclide species in waters, soils and sediments should therefore be essential for improving the prediction power of impact and risk assessment models. The present paper reviews available fractionation techniques which can be utilised for radionuclide speciation purposes.     

Comparative bioaccumulation kinetics of trace elements in Mediterranean marine sponges

While marine organisms such as bivalves, seagrasses and macroalgae are commonly used as biomonitors for the environment pollution assessment, widely distributed sponges received little attention as potential helpful species for monitoring programmes. In this study, the trace element and radionuclide bioaccumulation and retention capacities of some marine sponges were estimated in a species-comparative study using radiotracers technique. Six Mediterranean species were exposed to background dissolved concentrations of ^110mAg, ²⁴¹Am, ¹⁰⁹Cd, ⁶⁰Co, ¹³⁴Cs, ⁵⁴Mn, ⁷⁵Se and ⁶⁵Zn allowing the assessment of the uptake and depuration kinetics for selected elements. Globally, massive demosponges Agelas oroides, Chondrosia reniformis and Ircinia variabilis displayed higher concentration factor (CF) than the erectile ones (Acanthella acuta, Cymbaxinella damicornis, Cymbaxinella verrucosa) at the end of exposure, suggesting that the morphology is a key factor in the metal bioaccumulation efficiency. Considering this observation, two exceptions were noted: (1) A. acuta reached the highest CF for ^110mAg and strongly retained the accumulated metal without significant Ag loss when placed in depuration conditions and (2) C. reniformis did not accumulate Se as much as A. oroides and I. variabilis. These results suggest that peculiar metal uptake properties in sponges could be driven by specific metabolites or contrasting biosilification processes between species, respectively. This study demonstrated that sponges could be considered as valuable candidate for biomonitoring metal contamination but also that there is a need to experimentally highlight metal-dependant characteristic among species.     

Contribution to a more realistic approach in assessing the release of C-14 from low-level radioactive waste repositories

The contribution of C-14 to radiation exposure in the biosphere can be significant as compared to that of other radionuclides disposed in a repository for low-level radioactive waste. The release pathways of C-14 and processes relevant to its release from a closed final repository for low-level radioactive waste are discussed. Because a conservative approach may lead to undue overestimation of the potential radiation exposure, a more realistic approach is outlined. At the present level of refinement, our approach helps to provide a sufficient safety margin to German dose limits for radiation exposure of 0.3 mSv and can thus facilitate licence approval.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: “mobile” species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides (³H, ¹⁴C, ³⁶Cl, ⁹⁹Tc and ¹²⁹I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and ³⁶Cl showed little evidence of retardation, while the transport of ¹⁴C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially ⁹⁹Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of ¹²⁹I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some “mobile” radionuclides (especially ⁹⁹Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

Modelling radionuclide distribution and transport in the environment

Mathematical models of radionuclide distribution and transport in the environment have been developed to assess the impact on people of routine and accidental releases of radioactivity from a variety of nuclear activities, including: weapons development, production, and testing; power production; and waste disposal. The models are used to estimate human exposures and doses in situations where measurements have not been made or would be impossible or impractical to make. Model results are used to assess whether nuclear facilities are operated in compliance with regulatory requirements, to determine the need for remediation of contaminated sites, to estimate the effects on human health of past releases, and to predict the potential effects of accidental releases or new facilities. This paper describes the various applications and types of models currently used to represent the distribution and transport of radionuclides in the terrestrial and aquatic environments, as well as integrated global models for selected radionuclides and special issues in the fields of solid radioactive waste disposal and dose reconstruction. Particular emphasis is placed on the issue of improving confidence in the model results, including the importance of uncertainty analysis and of model verification and validation.     

Solute transport in crystalline rocks at Äspö — II: Blind predictions, inverse modelling and lessons learnt from test STT1

Based on the results from detailed structural and petrological characterisation and on up-scaled laboratory values for sorption and diffusion, blind predictions were made for the STT1 dipole tracer test performed in the Swedish Äspö Hard Rock Laboratory. The tracers used were nonsorbing, such as uranine and tritiated water, weakly sorbing ²²Na⁺, ⁸⁵Sr²⁺, ⁴⁷Ca²⁺and more strongly sorbing ⁸⁶Rb⁺, ¹³³Ba²⁺, ¹³⁷Cs⁺.Our model consists of two parts: (1) a flow part based on a 2D-streamtube formalism accounting for the natural background flow field and with an underlying homogeneous and isotropic transmissivity field and (2) a transport part in terms of the dual porosity medium approach which is linked to the flow part by the flow porosity.The calibration of the model was done using the data from one single uranine breakthrough (PDT3). The study clearly showed that matrix diffusion into a highly porous material, fault gouge, had to be included in our model evidenced by the characteristic shape of the breakthrough curve and in line with geological observations.After the disclosure of the measurements, it turned out that, in spite of the simplicity of our model, the prediction for the nonsorbing and weakly sorbing tracers was fairly good. The blind prediction for the more strongly sorbing tracers was in general less accurate. The reason for the good predictions is deemed to be the result of the choice of a model structure strongly based on geological observation. The breakthrough curves were inversely modelled to determine in situ values for the transport parameters and to draw consequences on the model structure applied. For good fits, only one additional fracture family in contact with cataclasite had to be taken into account, but no new transport mechanisms had to be invoked. The in situ values for the effective diffusion coefficient for fault gouge are a factor of 2–15 larger than the laboratory data. For cataclasite, both data sets have values comparable to laboratory data. The extracted K_d values for the weakly sorbing tracers are larger than Swedish laboratory data by a factor of 25–60, but agree within a factor of 3–5 for the more strongly sorbing nuclides. The reason for the inconsistency concerning K_ds is the use of fresh granite in the laboratory studies, whereas tracers in the field experiments interact only with fracture fault gouge and to a lesser extent with cataclasite both being mineralogically very different (e.g. clay-bearing) from the intact wall rock.     

Modelling multiple dispersion of radionuclides through the environment

The migration of a contaminant through the environment is the result of the transport by a variety of biotic and abiotic carriers which move according to different dispersion mechanisms. Consequently, the patterns of the distribution of a pollutant in the environment cannot be ever explained on the basis of a single migration process or assuming that the concentrations of contaminant in the different kinds of carriers quickly reach the equilibrium condition. The present work discusses two examples (wash-off from catchments and transport through soils of radionuclides) that clearly demonstrate the inadequacy of “single dispersion” models to predict these patterns. On the contrary, models based on multiple dispersion can successfully simulate the particular features of the above mentioned processes. It was demonstrated that the time behaviour of radionuclide migration rates from catchment of different rivers vary within small ranges as a consequence of multiple dispersion. This result can be useful for the development of generic predictive models.     

Using fallout plutonium as a probe for erosion assessment

A study has been carried out to assess the potential of using fallout plutonium (Pu), which originated from atmospheric nuclear-weapons tests, as a tool to investigate recent erosional processes within the lower Cotter water-supply catchment in the Australian Capital Territory. This catchment, which was predominantly pine plantation, was severely affected by a major bush fire in 2003. Accelerator mass spectrometry has been used to measure Pu in soil samples collected from a number of sites across the catchment. The results indicate that less than 1 cm of surface soil had been lost since the early 1960s over much of the catchment. Areas of more erodible soil have, however, lost 2-4 cm of topsoil, and a loss of ∼6 cm of soil was identified at one particular site.